The main objective is to determine compositional and structural details of the inorganic phase in teeth and bones. Infrared and Raman spectroscopy, x-ray diffraction and chemical methods are employed in these studies. A better understanding of the compositional and structural details of the apatite mineral phase in teeth and bones has been made possible by studies on its synthetic analogs. Consequently, methods are devised for the preparation of synthetic calcium apatites having controlled physical properties (crystal size and perfection) and chemical constituents (hydroxide, fluoride, chloride, carbonate, water, acid phosphate and other ions). The vibrational spectra of these apatites and related compounds are assigned and characterized. Isotopically enriched apatite analogs are prepared to facilitate spectral assignments. The spectroscopic assignments and supplemental spectral data (temperature dependence and polarization) are then utilized to establish compositional and structural details of the apatites in question, which include: the type and geometry of constituent ions; the site or number of sites occupied by the ions; orientation of ions; chemical bonding and interactions of ions; and semi-quantitative estimations of the constituents present. The results for these controlled apatite systems are then related to the inorganic phase in calcified tissues.